GREEN CHEMISTRY
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2026
·
IF 10.6
Zhenbang Liu,Shenghui Zhou,Jiangang Wang,Jinghua Wang,Hongyou Cui
The efficient conversion of cellulose into levulinic acid (LA) is a challenge due to the recalcitrant crystalline structure of cellulose and the facile formation of humin during the conversion process. Herein, we report a highly efficient and green catalytic system, which is composed of LiCl·3H2O (molten salt hydrate, MSH) and a bifunctional NbP/HZSM-5 catalyst, achieving a LA yield of 85.8% from microcrystalline cellulose (MCC) under mild conditions. Mechanistic investigation indicates that MSH not only helps disrupt the cellulose crystallinity but also serves as a co-catalyst to promote catalytic activity of NbP/HZSM-5. Their synergistic effect markedly lowers the activation energy of the 5-hydroxymethyl furfural (HMF)-to-LA reaction. Moreover, MSH can activate the produced LA and formic acid (FA) as an autocatalytic proton shuttle to form a self-accelerating cycle, which drastically reduces the dependence on external acid inputs. In addition, the catalytic system demonstrates excellent recyclability, still maintaining an 82.1% LA yield after four cycles. This research not only offers an efficient route for LA production from cellulose but also exemplifies a green chemistry-advancing strategy by integrating benign solvents, recyclable catalysts, and atom-efficient autocatalysis which align with the core principles of green chemistry.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2025
·
IF 2.8
Xiang Sun,Huilin Hu,Ning Kang,Zhenbiao Song,Shulai Lu,Songyang Huang,Shicheng Zhao
The research on ester-based lubricants for acrylonitrile–butadiene–styrene (ABS) resins has not yet received enough attention, and the structure–property relationship remains unknown. In this paper, 1,11-undecanediol levulinate (LAUD) and its ketalized derivative (K-LAUD) were successfully prepared as two ester-based lubricants for ABS, and the influence of the end-group structure on the lubrication properties was thoroughly evaluated. Both ABS/LAUD and ABS/K-LAUD were prepared by extrusion. Compared with ABS/LAUD, ABS/K-LAUD exhibited significantly lower glass transition temperature ( T g ), complex viscosity, and surface roughness. The tensile test results suggested that the elongation at break of ABS/K-LAUD increased by 23.3% compared to ABS/LAUD. This revealed that K-LAUD with ketal end-groups displayed enhanced lubrication properties in ABS. The lubrication mechanism was further proposed with molecular dynamic simulations. This could be primarily attributed to the unique ketal structure of K-LAUD, which offered abundant nucleophilic sites and a stronger binding energy with the polymer matrix. Furthermore, the presence of the 1,3-dioxane ring remarkably enlarged the free volume of the matrix and facilitated the molecular chain disentanglement, thus resulting in improved mobility and diffusivity of molecular chains. This work filled the research gap of structure–property relationships of ester-based lubricants for ABS and provided an academic foundation for the design of ester-based lubricants.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Meng-xing Xu,Yan Xu,Yu-zhen Liu,Dan Zhao,Shun-min Ding,Chao Chen
Acquiring practical catalysts was crucial for promoting the application of advanced chemical transformations. Here, a series of Co-Ni-P catalysts with addition of Y were designed for hydrogenation transformation of biomass-derived levulinic acid (LA) or furfural (FAL) in water. The molar-composition-manipulated catalysts were characterized in Co-Ni phosphide alloy nanostructure with YPO 4 enriched on surface and denoted as (YPO 4 ) x /Co y Ni 2-y P. By comprehensive catalytic measurements, both Co:Ni ratio in phosphide alloy and amount of YPO 4 were testified to be key factors to modulate intrinsic catalytic properties (hydrogen activation and acid catalysis) along Y-Co-Ni-P interface, the attractive and reproducible yield for desired product γ-valerolactone (up to 98 %) or cyclopentanone (up to 93%) could achieve under low H 2 pressure of 0.1–0.5 MPa over the well modulated catalyst (YPO 4 ) 0.2 /Co 1.0 Ni 1.0 P in comparison with high H 2 pressure (beyond 1.0 MPa) required in most of literature systems, indicating that the efficiency and feasibility of these important biomass transformations could be greatly enhanced on the low-cost and robust (YPO 4 ) x /Co y Ni 2-y P catalysts. These findings suggested that the phosphide-alloy engineering technique provided in this work could serve as a novel and practical method for innovating competitive catalysts to boost advanced heterogeneous catalysis applications as well as current aqueous hydrogenation transformations of biomass derivatives.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 38
·16526-16536
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IF 3.288
Xufeng Bai,Ting Ren,Jingbo Mao,Shenmin Li,Jingmei Yin,Jinxia Zhou
Cellulose-derived levulinic acid (LA) can be converted into gamma-valerolactone (GVL), a sustainable platform chemical for the production of bio-based chemicals. However, LA as an organic acid causes severe metal leaching during the heterogeneous hydrogenation of LA to GVL, especially in the presence of water. Various endeavors for preventing metal leaching have focused more on the process and less on the intrinsic nature of catalysts. The aim of this work is to derive a novel metal-leaching-resistant catalyst for the aqueous-phase hydrogenation of LA into GVL by using a nanocomposite containing three components, Ag, ZrO2, and graphene oxide (GO). The AgZrO2GO catalyst without pre-reduction treatment resulted in complete conversion of LA and approximately 100 mol% selectivity to GVL in the aqueous reaction, and metal leaching from the catalyst was completely eliminated. The relationship between the catalytic performance and the distinct physicochemical properties of the catalyst was extensively discussed.
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高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2019
·Vol. 36
·期 5
·740-752
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IF 2.476
Gong Chen,Wei Junnan,Tang Xing,Zeng Xianhai,Sun Yong,Lin Lu
Biomass-derived levulinic acid (LA) and its esters are currently envisaged as versatile, renewable platform chemicals. In this study, cellulosic pulp derived from the cooking of lignocellulosic biomass with active oxygen and solid alkali was employed as raw material for the formation of LA or ethyl levulinate (EL). This pretreatment process is highly effective for the delignification and deconstruction of lignocellulose matrix, making a facile degradation of the resulting cellulosic pulp to LA or EL. At this point, the acid-catalyzed hydrolysis or ethanolysis of cellulosic pulp was optimized by response surface methodology (RSM), offering desirable LA yield of 65.3% or EL yield of 62.7%, which is significantly higher than those obtained from raw biomass. More importantly, coking behavior on the inwall of the reactor was eliminated during the hydrolysis or ethanolysis of cellulosic pulp, which is one of the top challenges for the acid-catalyzed conversion of biomass in an industrial scale.
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GREEN CHEMISTRY
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2019
·Vol. 21
·期 16
·4499-4511
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IF 9.405
Yuewen Shao,Kai Sun,Qingyin Li,Qianhe Liu,Shu Zhang,Qing Liu,Guangzhi Hu,Xun Hu
γ-Valerolactone (GVL) and 1,4-pentanediol (1,4-PDO) are value-added chemicals that can be produced from levulinic acid/ester via hydrogenation coupled with acid/base-catalyzed reactions. In this study, we demonstrate that the Cu-based catalysts produced via the hydrotalcite precursors with tunable distribution of acidic and basic sites could, according to the requirement of the target products, effectively tune the production of GVL or to 1,4-PDO from levulinic acid/ester. The abundant Brønsted acid sites over the CuAl catalyst suppressed the opening of the ring of GVL, achieving a higher GVL selectivity while inhibiting 1,4-PDO formation. The introduction of Mg species to the catalyst significantly increased the abundance of the basic sites on the surface of the catalyst, which was essential for the selective conversion of GVL to 1,4-PDO via the opening of the ring structure of GVL, the rate-determining step in the conversion from levulinic acid/ester to 1,4-PDO. In addition, the CuMgAl catalyst showed a much superior catalytic stability to the CuMg or CuAl catalyst due to the more stable crystal structure, the more developed porous structure, the higher dispersion of the Cu species and the higher capability to suppress the growth of metallic Cu species under hydrothermal conditions.
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Catalysts
·
2015
·Vol. 5
·期 4
·1636-1648
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IF 2
Rui Wang,Xiaolin Xie,Yanxiu Liu,Zhigang Liu,Guofang Xie,Ning Ji,Lizhi Ma,Mingquan Tang
The kiwifruit industry is booming worldwide. As a result, a great deal of kiwifruit waste residue (KWR) containing monosaccharides is produced and discarded. This material shows great potential for the production of platform chemicals. In this study, a series of Nb/Al oxide catalysts were synthesized via a facile and low-cost coprecipitation method, and their structures were characterized using: thermal gravimetric analysis (TGA), XRD, FESEM, TEM, X-ray photoelectron spectroscopy (XPS), NH3-TPD, N2adsorption-desorption, and FTIR-Pyridine adsorption. Experimental results of sugar-to-levulinic acid (LA) conversion revealed that the 20%Nb/Al oxide catalyst provided the highest catalytic performance and durability in terms of LA yield from fructose (74.2%) at 463 K after 10 min and from glucose (47.5%) at 473 K after 15 min. Notably, the 20% Nb/Al oxide catalyst with a 10% dosage is capable of converting kiwifruit waste residue to LA at 473 K after 10 min. In conclusion, the enhanced catalytic performance was obtained due to the high acidity, and large surface areaof Nb/Al oxide catalyst.Keywords:levulinic acid;kiwifruit waste residue (KWR);heterogeneous catalysis;Nb/Al oxide catalyst
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GREEN CHEMISTRY
·
2016
·Vol. 18
·期 11
·3370-3377
·
IF 8.506
Wenjing Yang,Haiyang Cheng,Bin Zhang,Yan Li,Tong Liu,Mingli Lan,Yancun Yu,Chao Zhang,Weiwei Lin,Shin-ichiro Fujita,Masahiko Arai,Fengyu Zhao
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was studied with a homogeneous RuCl2(PPh3)3 catalyst in supercritical CO2 (scCO2). The conversion of LA was observed to increase with CO2 pressure and the possible reasons for this rate acceleration were discussed, including the molecular interactions of CO2 with the reacting and catalytic species as well as the acidity and phase behavior of the reaction mixture. The interaction between CO2 and RuCl2(PPh3)3 was significant, which resulted in the production of an active RuHCl(CO)(PPh3)3 complex and thus enhanced the rate of hydrogenation in the presence of CO2.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Ni Wei,Xin Xu,Jiushun Qin,Wei Lai,Ruoyan Li,Chenhuan Lai,Qiang Yong
Development of green pretreatment strategies with excellent lignin removal ability is particularly important for masson pine biorefinery. γ-Valerolactone (GVL), as a green and recyclable solvent, has unique solvent characteristics to extract lignin. In this study, three acid catalysts, including sulfuric acid (H 2 SO 4 ), hydrochloric acid (HCl) and p -toluenesulfonic acid (TsOH), were used to catalyze γ-valerolactone (GVL) pretreatment of masson pine. Among them, the TsOH-catalyzed GVL pretreatment achieved the highest lignin removal ratio and the best cellulose enzymatic hydrolysis yield. Under the optimized pretreatment conditions (150 ℃, 150 mM TsOH, GVL/H 2 O (4:1, w/w), 1 h), the lignin removal ratio reached 89.0 %, achieving a 72 h glucose yield of 87.1 % from the pretreated residues. The solvent lignins from pretreatment liquid was separated and characterized by NMR analysis. Meanwhile, the hexoses in pretreatment liquid were further converted into levulinic acid (LA) using the TsOH-catalyzed bi-phase reaction systems. This study gives insights into developing a biorefining process for the effective utilization of masson pine.
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Molecular Catalysis
·
2025
·
IF 4.9
Baoting Yi,Huimei Wang,Keyin Liu,Xiaohui Wang,Fangong Kong,Junli Ren
Catalytic biomass conversion is a crucial pathway for high-value utilization of renewable resources, yet current catalysts face limitations such as insufficient acid sites, poor product selectivity, and low cycling stability. This study developed a magnetic tin-based solid acid catalyst (Fe 3 O 4 @PDA-Sn) using 5-sulfoisophthalic acid sodium salt as a ligand and dopamine hydrochloride-coated Fe 3 O 4 for targeted catalytic conversion of sugarcane bagasse. Results demonstrated that the catalyst achieved a furfural yield of 86.2% and a levulinic acid yield of 32.5% at 170°C for 90 min, with FT-IR, NMR, and XRD confirming its differential deconstruction capability toward cellulose and hemicellulose. Mechanistic analysis demonstrated that the coordinated interaction between Brønsted and Lewis acid sites played a crucial role in steering the reaction toward specific pathways: hemicellulose hydrolysis products underwent dehydration to furfural (enriched in the organic phase), while cellulose was selectively cleaved to form levulinic acid. The catalyst maintained stable performance over 5 cycles without regeneration, with 97.3% magnetic recovery efficiency, offering a novel "facile magnetic separation–excellent cycling performance" strategy for hierarchical biomass conversion. This work provides critical insights into the design of multifunctional biorefinery catalysts for sustainable biomass valorization.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 10
·2805-2814
·
IF 3.709
Shuaibin Zhang,Bochao Yan,Zhihui Chen,Suping Zhang
BACKGROUND Levulinic acid, an important platform compound, is extensively used in textiles, dyes, antifreeze, animal feed, solvents and food additives. However, the use of lignocellulosic biomass to produce levulinic acid is difficult because of poor accessibility to cellulose and low hydrolytic yield. Thus a viable hydrolysis strategy and a suitable catalyst must be developed. RESULTS In this study, a bifunctional solid acid catalyst (HTC-SO 3 H) containing both cellulose binding sites ( Cl, COOH and OH) and catalytic sites ( SO 3 H) was prepared by a carbonization–grafting–oxidization method. X-ray photoelectron spectroscopy and Fourier transform infrared characterization confirmed the existence of Cl and the successful modification of the SO 3 H grafted hydrothermal carbon. The hydrogen bonds formed between cellulose and the binding sites ( Cl, OH and COOH) in the catalyst showed synergistic effects with the catalytic sites ( SO 3 H), leading to efficient hydrolysis of the furfural residue. A total of 74.81% (non-magnetic) and 70.18% (magnetic) levulinic acid yields were obtained after hydrolysis at 190 °C and 180 min in γ-valerolactone–H 2 O (1:1, v/v). Magnetic catalysts were synthesized using a co-precipitation method. Catalysts were recycled without any obvious reduction in catalytic activity. CONCLUSION Using sucralose as a raw material, the as-synthesized bifunctional solid acid catalyst improved the accessibility to cellulose and increased levulinic acid yield. Moreover, the grafted SO 3 H formed by hydroxyl hydration condensation exhibited superior stability. This study provides a valuable strategy for the efficient hydrolysis of lignocellulosic biomass. © 2022 Society of Chemical Industry (SCI).
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Wenxiu Cao,Lu Lin,Haifeng Qi,Qian He,Zhijie Wu,Aiqin Wang,Wenhao Luo,Tao Zhang
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction for the production of renewable chemicals and fuels, wherein acid-resistant and robust catalysts are highly desired for practical usage. Herein, an ultra-stable 0.6 wt% Ir@ZrO 2 @C single-atom catalyst was prepared via an in-situ synthesis approach during the assembly of UiO-66, followed by confined pyrolysis . The Ir@ZrO 2 @C offered not only a quantitative LA conversion and an excellent GVL selectivity (>99%), but also an unprecedented stability during recycling runs under harsh conditions (at T = 453 K, P H2 = 40 bar in pH = 3 or pH = 1 aqueous solution). By thorough spectroscopy characterizations, a well-defined structure of atomically dispersed Ir δ+ atoms onto nano-tetragonal ZrO 2 confined in the amorphous carbon was identified for the Ir@ZrO 2 @C. The strong metal-support interaction and the confinement of the amorphous carbon account for the ultra-stability of the Ir@ZrO 2 @C.
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